CAREER: Theoretical Analysis of Molecular Oxygen Chemistry in Biological Systems

威斯康星州大学的Qiang Cui通过CAREER奖获得理论和计算化学项目的支持，以开发和应用混合量子力学/分子力学方法来探索黄素蛋白中黄素-氧化学的细节。 具体而言，约束密度泛函理论将被用来构建非绝热态的黄素和分子氧之间的电子转移。 整体平均密度泛函理论将用于实现平衡的描述三重态和单重态的黄素-超氧自由基对进行自旋禁戒过渡。 这些方法可以扩展到与涉及分子氧的其他化学过程相关的能量学和动力学性质。 此外，充分互动，多媒体材料将开发计算生物物理课程，沿着一个基于网络的数据库的经典研究论文具有很大的教学价值。理论分析是非常有价值的，在确定详细的机制，并提供深入了解蛋白质活性位点环境的结构和动力学性质，特别是当实验本身是不确定的。 该研究项目将扩大酶模拟的范围和细节水平，超越传统的计算方法。 此外，新的多媒体教材和网上数据库将通过兼顾现代发展和基本概念，改善学生的学习体验。

Qiang Cui of the University of Wisconsin is supported by the Theoretical and Computational Chemistry Program through a CAREER award to develop and apply hybrid quantum mechanical/molecular mechanical methods to explore details of flavin-oxygen chemistry in flavoproteins. Specifically, a constrained density functional theory will be used to construct diabatic states relevant to electron transfer between flavin and molecular oxygen. Ensemble-averaged density functional theory will be used to achieve a balanced description of both triplet and singlet electronic states of the flavin-superoxide radical pair undergoing a spin-forbidden transition. These methods can be extended to the energetics and kinetic properties associated with other chemical processes involving molecular oxygen. In addition, fully interactive, multimedia material will be developed for computational biophysics courses, along with a web-based database of classic research papers with great pedagogical value.Theoretical analysis is very valuable in identifying detailed mechanisms and providing insights into the structural and dynamical properites of protein active site environments, especially when experiments alone are inconclusive. This research project will expand the scope and level of detail for enzyme simulations beyond what conventional computational methods offer. In addition, new multimedia course material and a web-based database will improve the student learning experience by incorporating a balance of modern developments and fundamental concepts.